Thermodynamic Mechanisms of Co-S Bond Anchoring in Few-Layered 1T-MoS₂ for Enhanced Capacitive Performance via Spin State Regulation and Ion Diffusion Kinetics

Abstract

Few-layered 1T-MoS₂ is highly promising for supercapacitor applications due to its wide interlayer spacing, high electrical conductivity, and abundant active sites. However, its poor structural stability greatly challenges the synthesis of stable 1T-MoS₂. This study systematically investigates the dual-function mechanism of cobalt (Co) doping in few-layered MoS₂. Co is successfully doped into MoS₂ to fabricate stable 1T-MoS₂ by a simple synthesis approach. The formation of Co-S bonds during doping plays a critical role in stabilizing the 1T phase. Furthermore, Co doping deliberately induces defects in the MoS₂ lattice. The defects modify the electronic structure, increasing the density of states near the Fermi level, and enhancing both electrical conductivity and charge-transfer efficiency. SEM, XRD, and XPS characterizations of samples stored for half a year show that Co doping stabilizes the morphology and crystal phase of 1T-MoS₂. DFT calculations further validate the enhanced performance of Co doping MoS₂. Specifically, M-Co (1.5%) (1.5% Co-MoS₂) reaches a specific capacitance of 197 F g⁻¹ at 1 A g⁻¹, with 88% capacitance retention after 40 000 cycles. The assembled M-Co (1.5%)//CC asymmetric supercapacitor device maintains 92% capacity retention after 20 000 cycles. This work offers new insights into stable 1T-MoS₂ preparation and promotes the application of TMDs in supercapacitors.

Keywords

asymmetric supercapacitor device / cyclic stability / doping / few-layered 1T-MoS₂ / supercapacitor

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2026 The Author(s). Energy & Environmental Materials published by John Wiley & Sons Australia, Ltd on behalf of Zhengzhou University.